Carbon capture and storage (CCS) has been recognized as a pivotal technology for mitigating climate change by reducing CO2 emissions. Storing CO2 in deep saline aquifers requires preserving the water-wet nature of the formation throughout the storage period, which is crucial for maintaining rock integrity and storage efficiency. However, the wettability of formations can change upon exposure to supercritical CO2 (scCO2), potentially compromising storage efficiency. Despite extensive studies on various factors influencing wettability alteration, a significant research gap remains in understanding the effects of different CO2 injection strategies on wettability in deep saline formations (DSFs). This study addresses this gap by investigating how three distinct CO2 injection strategies—continuous scCO2 injection (CCI), water alternating with scCO2 injection (WAG), and simultaneous water and scCO2 injection (SAI)—affect the wettability of gray Berea sandstone and Indiana limestone, both selected for their homogeneous properties relevant to CCS. Using a standardized sessile drop contact angle method before and after CO2 injection, along with core flooding to model the injection process at an injection pressure of 1500 psi and temperature of 100 °F with a confining pressure of 2500 psi, the results indicate a shift in wettability towards more CO2-wet conditions for both rock types under all strategies with changes in CA of 61.6–83.4° and 77.6–87.9° and 81.5–124.2° and 94.6–128.0° for sandstone and limestone, respectively. However, the degree of change varies depending on the injection strategy: sandstone exhibits a pronounced response to the CCI strategy, with up to a 77% increase in contact angle (CA), particularly after extended exposure. At the same time, WAG shows the least change, suggesting that water introduction slows surface modification. For limestone, the changes in CA ranged from 9% to 49% across strategies, with WAG and SAI being more effective in altering its wettability. This study underscores the importance of selecting suitable CO2 injection strategies based on rock type and wettability characteristics to maximize carbon storage efficiency. The findings offer valuable insights into the complex interactions of fluid–rock systems and a guide for enhancing the design and implementation of CCS technologies in various geological settings.
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